Origin of rate limitations in solid-state polymer batteries from constrained segmental dynamics within the cathode

X. Chelsea Chen; Charles Soulen; Mary K. Burdette-Trofimov; Xiaomin Tang; Changhao Liu; Luke Heroux; Mathieu Doucet; Madhusudan Tyagi; Gabriel M. Veith

doi:10.1016/j.xcrp.2023.101538

Origin of rate limitations in solid-state polymer batteries from constrained segmental dynamics within the cathode

X. Chelsea Chen, Charles Soulen, Mary K. Burdette-Trofimov, Xiaomin Tang, Changhao Liu, Luke Heroux, Mathieu Doucet, Madhusudan Tyagi, Gabriel M. Veith

Research output: Contribution to journal › Article › peer-review

Abstract

Currently, one of the key challenges preventing the wide commercialization of polymer-based solid-state batteries is achieving high-rate capabilities. This work unravels chain structure and segmental dynamics in a polymer-based composite cathode consisting of LiFePO₄ (LFP), carbon, and poly(ethylene oxide) (PEO) with lithium bis(trifluoromethanesulfonyl)imide. Small-angle neutron scattering (SANS) data reveal that PEO chains are adsorbed on the surface of LFP particles during slurry processing to make the composite electrode. The strong interaction between LFP and PEO chains leads to greatly reduced segmental dynamics of PEO, as discovered by quasi-elastic neutron scattering (QENS). The reduced segmental dynamics results in 70% decreased Li⁺ mobility of the polymer electrolyte in the composite cathode. The combined SANS and QENS study indicates that one of the key bottlenecks that limits the rate performance of PEO-based polymer batteries originates from molecular interactions within the cathode.

Original language	English
Article number	101538
Journal	Cell Reports Physical Science
Volume	4
Issue number	8
DOIs	https://doi.org/10.1016/j.xcrp.2023.101538
State	Published - Aug 16 2023

Funding

This work was completed with funds from the Department of Energy’s Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s US-German Cooperation on Energy Storage: Cathode-Solid-Electrolyte Interfaces program. This work was initiated with the support from the US Department of Energy , Office of Science , Basic Energy Sciences , Materials Science and Engineering Division . Work at ORNL’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division , Office of Basic Energy Sciences , US Department of Energy (L.H., M.D.). Access to the HFBS was provided by the Center for High Resolution Neutron Scattering , a partnership between the National Institute of Standards and Technology and the National Science Foundation under Agreement No. DMR-2010792 . The identification of any commercial product or trade name does not imply endorsement or recommendation by the National Institute of Standards and Technology (NIST).

Funders	Funder number
Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office
Scientific User Facilities Division
National Science Foundation	DMR-2010792
U.S. Department of Energy
National Institute of Standards and Technology
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Division of Materials Sciences and Engineering

Keywords

cathode
ion transport
lithium
polymer electrolyte
quasi-elastic neutron scattering
segmental dynamics
small-angle neutron scattering
solid-state battery

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.xcrp.2023.101538

Cite this

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title = "Origin of rate limitations in solid-state polymer batteries from constrained segmental dynamics within the cathode",

abstract = "Currently, one of the key challenges preventing the wide commercialization of polymer-based solid-state batteries is achieving high-rate capabilities. This work unravels chain structure and segmental dynamics in a polymer-based composite cathode consisting of LiFePO4 (LFP), carbon, and poly(ethylene oxide) (PEO) with lithium bis(trifluoromethanesulfonyl)imide. Small-angle neutron scattering (SANS) data reveal that PEO chains are adsorbed on the surface of LFP particles during slurry processing to make the composite electrode. The strong interaction between LFP and PEO chains leads to greatly reduced segmental dynamics of PEO, as discovered by quasi-elastic neutron scattering (QENS). The reduced segmental dynamics results in 70% decreased Li+ mobility of the polymer electrolyte in the composite cathode. The combined SANS and QENS study indicates that one of the key bottlenecks that limits the rate performance of PEO-based polymer batteries originates from molecular interactions within the cathode.",

keywords = "cathode, ion transport, lithium, polymer electrolyte, quasi-elastic neutron scattering, segmental dynamics, small-angle neutron scattering, solid-state battery",

author = "Chen, {X. Chelsea} and Charles Soulen and Burdette-Trofimov, {Mary K.} and Xiaomin Tang and Changhao Liu and Luke Heroux and Mathieu Doucet and Madhusudan Tyagi and Veith, {Gabriel M.}",

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doi = "10.1016/j.xcrp.2023.101538",

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AU - Chen, X. Chelsea

AU - Soulen, Charles

AU - Burdette-Trofimov, Mary K.

AU - Tang, Xiaomin

AU - Liu, Changhao

AU - Heroux, Luke

AU - Doucet, Mathieu

AU - Tyagi, Madhusudan

AU - Veith, Gabriel M.

PY - 2023/8/16

Y1 - 2023/8/16

N2 - Currently, one of the key challenges preventing the wide commercialization of polymer-based solid-state batteries is achieving high-rate capabilities. This work unravels chain structure and segmental dynamics in a polymer-based composite cathode consisting of LiFePO4 (LFP), carbon, and poly(ethylene oxide) (PEO) with lithium bis(trifluoromethanesulfonyl)imide. Small-angle neutron scattering (SANS) data reveal that PEO chains are adsorbed on the surface of LFP particles during slurry processing to make the composite electrode. The strong interaction between LFP and PEO chains leads to greatly reduced segmental dynamics of PEO, as discovered by quasi-elastic neutron scattering (QENS). The reduced segmental dynamics results in 70% decreased Li+ mobility of the polymer electrolyte in the composite cathode. The combined SANS and QENS study indicates that one of the key bottlenecks that limits the rate performance of PEO-based polymer batteries originates from molecular interactions within the cathode.

AB - Currently, one of the key challenges preventing the wide commercialization of polymer-based solid-state batteries is achieving high-rate capabilities. This work unravels chain structure and segmental dynamics in a polymer-based composite cathode consisting of LiFePO4 (LFP), carbon, and poly(ethylene oxide) (PEO) with lithium bis(trifluoromethanesulfonyl)imide. Small-angle neutron scattering (SANS) data reveal that PEO chains are adsorbed on the surface of LFP particles during slurry processing to make the composite electrode. The strong interaction between LFP and PEO chains leads to greatly reduced segmental dynamics of PEO, as discovered by quasi-elastic neutron scattering (QENS). The reduced segmental dynamics results in 70% decreased Li+ mobility of the polymer electrolyte in the composite cathode. The combined SANS and QENS study indicates that one of the key bottlenecks that limits the rate performance of PEO-based polymer batteries originates from molecular interactions within the cathode.

KW - cathode

KW - ion transport

KW - lithium

KW - polymer electrolyte

KW - quasi-elastic neutron scattering

KW - segmental dynamics

KW - small-angle neutron scattering

KW - solid-state battery

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ER -

Origin of rate limitations in solid-state polymer batteries from constrained segmental dynamics within the cathode

Abstract

Funding

Keywords

UN SDGs

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